在二维合金属-有机框架中对金属和连接物的修饰用于CO2电还原:密度函数理论和机器学习研究的联合密度
Guanru Xing1, Shize Liu2, Guang-Yan Sun3
1Laboratory of Theoretical and Computational Chemistry, Institute of Theoretical Chemistry, College of Chemistry, Jilin University, Changchun 130023, China.
Journal of colloid and interface science
|August 13, 2024
概括
本研究探讨了用于电化学二氧化碳减排的二维合金属有机框架 (2D c-MOFs). 六种新型催化剂在CO,HCOOH和CH4生产方面表现出卓越的性能,性能优于传统的铜催化剂.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 计算化学计算化学
背景情况:
- 电化学二氧化碳还原反应 (CO2RR) 对人工碳循环至关重要.
- 由于高电导率,二维结合金属有机框架 (2D c-MOF) 显示出作为高效的催化剂的前景.
研究的目的:
- 设计和系统地研究一系列2D c-MOFs (TMNxO4-x-HDQ) 的CO2RR.
- 为特定的CO2RR产品识别具有高活性和选择性的催化剂.
- 使用计算方法了解控制CO2RR性能的内在因素.
主要方法:
- 用密度函数理论 (DFT) 的计算来研究37个设计的二维c-MOF的催化性能.
- 评估了MOF的热力学和电化学稳定性.
- 机器学习 (ML) 分析被用来确定CO2RR活动的关键描述符.
主要成果:
- 所有设计的TMNxO4-x-HDQ结构都表现出良好的稳定性.
- 六个催化剂在活性和选择性方面超过了Cu211表面.
- 对于二氧化碳的产生 (UL = -0.04 V),NiN4-HDQ的表现非常出色.
- CuN4-HDQ,NiN2O2-HDQ和PtN2O2-HDQ对HCOOH的产生是活跃的 (UL = -0.27到 -0.29 V).
- MnN4-HDQ和NiO4-HDQ显示出CH4生产的高活性 (UL = 分别为-0.58和-0.24V).
- 这些催化剂有效地抑制了进化反应.
- ML分析确定了电子亲和力,电子阴性,电离能,p波段中心,金属原子半径和d波段中心作为关键性能因素.
结论:
- 该研究成功地确定了CO2RR.的高活性和选择性的2D c-MOF电催化剂.
- 这些发现为有效的二氧化碳转化提供了对催化剂设计原则的宝贵见解.
- 开发的TMNxO4-x-HDQ材料为推进人工碳循环技术提供了一个有前途的平台.
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